Hydrogenation of Bio-Oil Oxygenates at Ambient Conditions via a Two-Step Redox Cycle

作     者：Ruan, Chongyan Akutsu, Ryota Yang, Kunran Zayan, Noha M. Dou, Jian Liu, Junchen Bose, Arnab Brody, Leo Lamb, H. Henry Li, Fanxing 

作者机构：Department of Chemical and Biomolecular Engineering North Carolina State University RaleighNC United States Chemistry and Materials Division Department of Textile Science and Technology Shinshu University Japan 

出 版 物：《SSRN》 

年 卷 期：2023年

核心收录：

主　　题：Hydrogenation 

摘      要：A key challenge in upgrading bio-oils to renewable fuels and chemicals resides in developing effective and versatile hydrogenation systems. Herein, we report a two-step solar thermochemical hydrogenation process that sources hydrogen directly from water and concentrated solar radiation for furfural and bio-oils upgrading. Superior catalytic performance was achieved at room temperature and atmospheric pressure, with up to two orders of magnitude higher H2 utilization efficiency compared to state-of-the-art catalytic hydrogenation. A metal or reduced metal oxide, obtainable from solar thermal or electrochemical reduction, provides the active sites for furfural adsorption and H2O dissociation. Fundamentally different from conventional hydrogenation, the in situ generated reactive H atoms hydrogenate furfural and biomass-derived oxygenates, eliminating the barriers for H2 dissolution and mass transfer in the reaction medium and the subsequent dissociation at the catalyst surface. The hydrogenation selectivity can be conveniently mediated by solvents with different polarity and metal/reduced metal oxide catalysts with varying oxophilicity, adding extra dimensions in manipulating the product distribution. This work provides an efficient and versatile strategy for bio-oils upgrading and a promising pathway for renewable energy storage. The generalized approach is also shown to be extendable to catalytic upgrading of other platform compounds with similar functional groups. © 2023, The Authors. All rights reserved.